(H,Li)$_{6}$Ru$_{2}$O$_{6}$ : a possible zero-field Ru$^{3+}$-based Kitaev Quantum Spin Liquid

TL;DR

This paper reports the synthesis of (H,Li)$_{6}$Ru$_{2}$O$_{6}$, a honeycomb Ru$^{3+}$ system that exhibits quantum spin liquid behavior without magnetic order, showing unique low-temperature and field-dependent properties consistent with Kitaev physics.

Contribution

It introduces a new Ru-based compound that demonstrates a zero-field Kitaev quantum spin liquid state, expanding the class of materials with such exotic magnetic properties.

Findings

No static magnetic moments or spin glass phase down to 84 mK.

Evidence of a crossover to a liquid-like state below 40 K.

Field-dependent scaling behaviors in NMR and heat capacity.

Abstract

We report the synthesis and properties of (H,Li)$_{6}$Ru$_{2}$O$_{6}$, which is shown to be a $J_{\text{eff}}=\frac{1}{2}$ system made out of Ru$^{3+}$ moments in a honeycomb geometry. Bulk magnetization, heat capacity, nuclear magnetic resonance (NMR), and muon spin relaxation ($\mu$SR) rule out the presence of static moments or any spin glass phase down to 84 mK. All techniques suggest a crossover to a liquid-like state below about 40 K. The $^{7}$Li nuclear magnetic resonance (NMR) shift data suggest a non-zero $T$-independent spin susceptibility at low $T$. In zero field, $C_m/T$ shows $T^{-0.9}$ divergence which is consistent with vacancy-induced effects on low-energy excitations of the pristine Kitaev spin liquid. With field, power-law variations in the $^{7}$Li NMR spin-lattice relaxation rate 1/T$_{1}$ and magnetic heat capacity $C_{m}$ show quantitatively new scaling behaviors. A two-step entropy release in heat capacity is also observed putatively from $Z_{2}$ flux (low-$T$ step) and itinerant Majorana fermions (high-$T$ step). Based on these findings, we propose that (H,Li)$_{6}$Ru$_{2}$O$_{6}$ realizes a Kitaev spin liquid with no evidence of inherent magnetic ordering in zero field unlike $\alpha$-RuCl$_{3}$ where approximately $8$ Tesla field is required to suppress magnetic order.